Microcomb spectral fingerprinting enables parts-per-trillion methane detection with low humidity cross-sensitivity
Optical frequency combs have transformed molecular spectroscopy by enabling broadband, high-resolution analysis, yet they are conventionally used as light sources to interrogate external samples. Here, we introduce an integrated microcomb sensing architecture that unifies resonantly enhanced evanescent sensing with multiwavelength molecular fingerprinting in a single ultrahigh-quality-factor silica microresonator. Gaseous analytes interact directly with the evanescent field of light recirculating within the resonator, enhancing sensitivity while encoding analyte-induced perturbations across the microcomb's collective spectral response. Rather than relying on a single optical resonance, we exploit distributed responses across multiple comb lines to generate multidimensional molecular fingerprints. Adding more comb lines systematically improves analyte discrimination, showing that the microcomb provides sensing information beyond what individual spectral channels offer. Using methane as a model analyte, we achieve an estimated detection limit of 178 parts per trillion, with minimal spectral responses to ammonia, carbon monoxide, hexane, and water vapor at relative humidities up to 90%. By replacing physically long interaction paths with resonant light recirculation in an ultrahigh-Q microresonator, this architecture brings compact optical sensing into the parts-per-trillion regime while exploiting distributed spectral information for chemical identification.